Cu-MOF-Derived Nano-Dendritic Self-Supported Electrodes for Efficient Electrochemical Nitrate-to-Ammonia Conversion

Electrochemical nitrate reduction reaction (eNO3RR) has emerged as a promising alternative to the energy-intensive and carbon-intensive Haber–Bosch process for green ammonia synthesis. However, the intrinsic complexity of the eight-electron transfer pathway and inevitable competing side reactions limit the activity and selectivity of eNO3RR. Maximizing the utilization of active sites and ensuring structural stability in electrocatalysts are essential for promoting surface proton-coupled electron transfer and improving Faradaic efficiency. Herein, we present a copper metal–organic framework (Cu-MOF)-derived electrocatalyst synthesized via in situ electrosynthesis on copper foam, using cetyltrimethylammonium bromide (CTAB) as a structure-directing agent, followed by electroreduction to produce a self-supported, nano-dendritic structure. This three-dimensional architecture exposes abundant active sites and facilitates electron transport, enabling efficient nitrate-to-ammonia conversion. The optimized CTAB-assisted electrode achieves an ammonia yield of 14.33 ± 0.61 mg h−1 cm−2 with a Faradaic efficiency of 90.95 ± 2.28% at −1.7 V versus Ag/AgCl. This study introduces a versatile design strategy for copper-based electrocatalysts that integrates structural stability with high activity, offering a sustainable approach for both ammonia production and nitrate remediation.